Electronic Interpretation of Interlayer Energy Landscape in Layered Materials

Abstract The interlayer energy landscape of layered materials is essential to disassemble their structure–property relationships. However, a clear definition of interlayer electronic coupling that generally rules the interlayer energy landscape for their outstanding electronic and tribological properties, remains a matter of debate. Herein, diverse methods for electron coupling are evaluated to discriminate their feasibility to interpret interlayer sliding energy landscape for frictional sliding or stacking faults, by using density functional theory calculation of the layered models in the case of transition metal dichalcogenides (TMDs). It is discovered that the charge density evolution in dynamic stacking configurations dictates the interlayer energy landscape along the sliding pathway, challenging the prevailing belief that the energy corrugation arises from the nonuniform distribution of charge density or the charge density in the interface region. The present studies may open the way to disassemble the electron coupling principle underlying interlayer energy landscape for structure–property relationships as stacking faults, registry effects, even superlubric behavior in layered structures.